“…Polyurethane has a unique microphase separation microstructure because of the poor thermodynamic compatibility between the hard segments and soft matrixes, which endows it with a remarkable toughness and elasticity. , On top of that, polyurethane architecture can be easily tailored by diols, isocyanates, and chain extenders, thus enabling the development of a series of derived materials with comprehensive properties. In the past few years, researchers have developed some high-performance and self-healable polyurethanes by introducing dynamic covalent bonds or supramolecular motifs into the molecular backbones, , for example, disulfide bond, , ĎâĎ stacking, metalâligand coordination, , and H-bond. â These reversible chemical bonds allow the as-prepared polyurethanes to be completely or partially repaired after being damaged. , It is particularly worth mentioning that the H-bond is an advisable interaction toward the preparation of self-healing macromolecules, due to the outstanding stability and rapid kinetic reversibility. , Intriguingly, it has been confirmed that abundant H-bond supramolecular interactions extensively exist in numerous biomacromolecules (titin, cellulose, , spider silk, â and so on), which manifest the efficient combination of mechanical robustness and self-healing capability. So far, many efforts have been devoted to mimicking these biopolymers to synthesize polyurethane materials with modulated properties.…”